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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 559 records · Page 31
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Atomic-Scale Insights into Surface Lattice Oxygen Activation at the Spinel/Perovskite interface of Co 3 O 4 /La 0.3 Sr 0.7 CoO 3

Surface lattice oxygen in transition-metal oxides plays a vital role in catalytic processes. Mastering activation of surface lattice oxygen and identifying the activation mechanism are crucial for the development and design of advanced catalysts. A strategy is now developed to create a spinel Co 3 O 4 /perovskite La 0.3 Sr 0.7 CoO 3 interface by in situ reconstruction of the surface Sr enrichment region in perovskite LSC to activate surface lattice oxygen. XAS and XPS confirm that the regulated chemical interface optimizes the hybridized orbital between Co 3d and O 2p and triggers more electrons in oxygen site of LSC transferred into lattice of Co 3 O 4 , leading to more inactive O 2- transformed into active O 2-x . Furthermore, the activated Co 3 O 4 /LSC exhibits the best catalytic activities for CO oxidation, oxygen evolution, and oxygen reduction. This work would provide a fundamental understanding to explain the activation mechanism of surface oxygen sites.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Metal–Metal Oxide Catalytic Interface Formation and Structural Evolution: A Discovery of Strong Metal–Support Bonding, Ordered Intermetallics, and Single Atoms

In-depth investigation of metal–metal oxide interactions and their corresponding evolution is of paramount importance to heterogeneous catalysis as it allows the understanding and maneuvering of the structure of catalytic motifs. Herein, using a series of core/shell metal/iron oxide (M/FeO x , M = Pd, Pt, Au) nanoparticles and through a combination of in situ and ex situ electron and X-ray investigations, we revealed anomalous and dissimilar M–FeO x interactions among different systems under reducing conditions. Further, Pd interacts strongly with FeO x after high-temperature reductive treatment, featured by the formation of Pd single atoms in the FeO x matrix and increased Pd–Fe bonding, while Pt transforms into ordered PtFe intermetallics and Pt single atoms immediately upon the coating of FeO x . In contrast, Au does not manifest strong bonding with FeO x . As a proof of concept of tailoring metal–metal oxide interactions for catalysis, optimized Pd/FeO x demonstrates 100% conversion and 86.5% selectivity at 60 °C for acetylene semihydrogenation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Effects of three-dimensional Cu/Nb interfaces on strengthening and shear banding in nanoscale metallic multilayers

Manipulation of the atomic-scale structure of two-dimensional (2D) interfaces have been shown to provide nanocomposites with enhanced strength, deformability, and radiation damage resistance. In comparison with 2D interfaces, here we investigate the mechanical response of nanocomposites containing three-dimensional (3D) Cu/Nb interfaces consisting of a chemical/structural gradient separating pure Cu and Nb layers, through which the lattice mismatch between face-centered cubic Cu and body-centered cubic Nb is accommodated over a distance of several nanometers. Furthermore, it is demonstrated that 3D interfaces increase the yield and flow strength by 50% and 22%, respectively, over composites containing 2D interfaces at similar layer thicknesses. After 14% compressive strain, the onset of shear banding results in co-deformation of both Cu and Nb phases within and outside of the shear band. We conclude with a discussion of the role of interface structure in shear band formation and growth in 3D Cu/Nb.

3-dimensional interface↗
DOE OSTI2015

STRUCTURE OF THE INTERSTELLAR BOUNDARY EXPLORER RIBBON FROM SECONDARY CHARGE-EXCHANGE AT THE SOLAR–INTERSTELLAR INTERFACE

In 2009, the Interstellar Boundary Explorer discovered a bright “ribbon” of energetic neutral atom (ENA) flux in the energy range ≤0.4–6 keV, encircling a large portion of the sky. This observation was not previously predicted by any models or theories, and since its discovery, it has been the subject of numerous studies of its origin and properties. One of the most studied mechanisms for its creation is the “secondary ENA” process. Here, solar wind ions, neutralized by charge-exchange with interstellar atoms, propagate outside the heliopause; experience two charge-exchange events in the dense outer heliosheath; and then propagate back inside the heliosphere, preferentially in the direction perpendicular to the local interstellar magnetic field. This process has been extensively analyzed using state-of-the-art modeling and simulation techniques, but it has been difficult to visualize. In this Letter, we show the three-dimensional structure of the source of the ribbon, providing a physical picture of the spatial and energy scales over which the secondary ENA process occurs. These results help us understand how the ribbon is generated and further supports a secondary ENA process as the leading ribbon source mechanism.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Effect of Near-Interface Compensation of CdSeTe Absorber Layers on Solar Cell Performance

Arsenic has been shown to be an effective p-type dopant of CdTe. However, challenges remain in the fabrication of high efficiency CdTe solar cells using As. As-doped CdTe is prone to self-compensation and observed accumulation of dopant atoms in CdTe near the interface with MgZnO (MZO) suggests that this could be occurring. In this study, we use SCAPS 1-D modeling software to investigate the effect of near-interface compensation. We consider three cases: shallow donors, deep recombination centers, and a thin layer of excess positive charge accumulation. All of these cases are shown to have significant effects on the current-voltage characteristics, while the thin charge layer also affects capacitance-voltage measurements.

arsenic↗
DOE OSTI2018

A Chain Model of a Zigzag Contact of Lateral Graphene-Like Heterostructures

A simple structural model is proposed for the zigzag interface formed by contacting two-dimensional graphene-like compounds AB and CD (both free and formed on a metal). For the graphene–hexagonal boron nitride system, analytical expressions for the electron spectrum, density of states, and atom occupation numbers at the interface are obtained. The results of calculating the densities of states and occupation numbers within two alternative approximations are in good agreement.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Temperature-controlled metal/ligand stoichiometric ratio in Ag-TCNE coordination networks

The deposition of tetracyanoethylene (TCNE) on Ag(111), both at Room Temperature (RT, 300 K) and low temperatures (150 K), leads to the formation of coordination networks involving silver adatoms, as revealed by Variable-Temperature Scanning Tunneling Microscopy. Our results indicate that TCNE molecules etch away material from the step edges and possibly also from the terraces, which facilitates the formation of the observed coordination networks. Moreover, such process is temperature dependent, which allows for different stoichiometric ratios between Ag and TCNE just by adjusting the deposition temperature. X-ray Photoelectron Spectroscopy and Density Functional Theory calculations reveal that charge-transfer from the surface to the molecule and the concomitant geometrical distortions at both sides of the organic/inorganic interface might facilitate the extraction of silver atoms from the step-edges and, thus, its incorporation into the observed TCNE coordination networks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Galvanic Replacement-Driven Transformations of Atomically Intermixed Bimetallic Colloidal Nanocrystals: Effects of Compositional Stoichiometry and Structural Ordering

Galvanic replacement reactions dictated by deliberately designed nanoparticulate templates have emerged as a robust and versatile approach that controllably transforms solid monometallic nanocrystals into a diverse set of architecturally more sophisticated multimetallic hollow nanostructures. The galvanic atomic exchange at the nanoparticle/liquid interfaces induces a series of intriguing structure-transforming processes that interplay over multiple time and length scales. Using colloidal Au–Cu alloy and intermetallic nanoparticles as structurally and compositionally fine-tunable bimetallic sacrificial templates, we show that atomically intermixed bimetallic nanocrystals undergo galvanic replacement-driven structural transformations remarkably more complicated than those of their monometallic counterparts. Here, we interpret the versatile structure-transforming behaviors of the bimetallic nanocrystals in the context of a unified mechanistic picture that rigorously interprets the interplay of three key structure-evolutionary pathways: dealloying, Kirkendall diffusion, and Ostwald ripening. By deliberately tuning the compositional stoichiometry and atomic-level structural ordering of the Au–Cu bimetallic nanocrystals, we have been able to fine-maneuver the relative rates of dealloying and Kirkendall diffusion with respect to that of Ostwald ripening through which an entire family of architecturally distinct complex nanostructures are created in a selective and controllable manner upon galvanic replacement reactions. The insights gained from our systematic comparative studies form a central knowledge framework that allows us to fully understand how multiple classic effects and processes interplay within the confinement by a colloidal nanocrystal to synergistically guide the structural transformations of complex nanostructures at both the atomic and nanoparticulate levels.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Catastrophic degradation of the interface of epitaxial silicon carbide on silicon at high temperatures

Epitaxial cubic silicon carbide on silicon is of high potential technological relevance for the integration of a wide range of applications and materials with silicon technologies, such as micro electro mechanical systems, wide-bandgap electronics, and graphene. The hetero-epitaxial system engenders mechanical stresses at least up to a GPa, pressures making it extremely challenging to maintain the integrity of the silicon carbide/silicon interface. In this work, we investigate the stability of said interface and we find that high temperature annealing leads to a loss of integrity. High–resolution transmission electron microscopy analysis shows a morphologically degraded SiC/Si interface, while mechanical stress measurements indicate considerable relaxation of the interfacial stress. From an electrical point of view, the diode behaviour of the initial p-Si/n-SiC junction is catastrophically lost due to considerable inter-diffusion of atoms and charges across the interface upon annealing. Temperature dependent transport measurements confirm a severe electrical shorting of the epitaxial silicon carbide to the underlying substrate, indicating vast predominance of the silicon carriers in lateral transport above 25 K. This finding has crucial consequences on the integration of epitaxial silicon carbide on silicon and its potential applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Substrate effects on phase formation and interfacial stability in superconducting vanadium silicide thin films

Thin films of vanadium silicide (V-silicide) in the A15 cubic phase (V 3 Si) are promising for superconducting quantum devices due to their high transition temperature and potential compatibility with scalable semiconductor fabrication. However, solid-phase synthesis often yields secondary silicide phases that degrade performance. Here, in this study, we investigate the influence of substrate properties using two silicon-on-insulator architectures: one with a polycrystalline HfO 2 buried layer (group A) and the other with amorphous SiO 2 (group B). Both systems exhibit superconductivity consistent with V 3 Si formation, yet structural analysis reveals mixed-phase films in both cases. Crucially, only group A maintains an atomically sharp and chemically stable interface, a prerequisite for phase purity. Prolonged annealing in group A reduces the unwanted V 5 Si 3 phase but also leads to the emergence of Si-rich VSi 2 , likely due to localized substrate degradation. Preliminary atomic-resolution imaging suggests that HfO 2 crystallinity may promote local phase-selective nucleation. These findings highlight the importance of substrate design in promoting phase control and maintaining interfacial integrity in superconducting silicides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Structural Rearrangement of Au–Pd Nanoparticles under Reaction Conditions: An ab Initio Molecular Dynamics Study

The structure, composition, and atomic distribution of nanoalloys under operating conditions are of significant importance for their catalytic activity. In the present work, ab initio molecular dynamics simulations are performed to understand the structural behavior of a Au-Pd nanoalloy supported on rutile TiO2 under different conditions. We find that the Au-Pd structure is strongly dependent on the redox properties of the support, originating from strong metal-support interactions. Under reducing conditions, Pd atoms are inclined to move toward the metal/oxide interface, evidenced by a significant increase of Pd-Ti bonds. This could be attributed to the charge localization at the interface that leads to Coulomb attractions to positively charged Pd atoms. In contrast, Pd atoms would rather stay inside the nanoparticle or on the alloy surface under oxidizing conditions. Moreover, Pd atoms on can be stabilized by hydrogen adsorption, forming Pd-H bonds, which are stronger than Au-H bonds. Our work provides an important insight into the structure design of Pd-Au nanoalloy catalyst and may lead to potential applications in dioxygen activation processes where Pd atoms are generally considered to be the active sites.

Xu, Cong-Qiao↗
DOE OSTI2017

In situ atomic-scale imaging of the metal/oxide interfacial transformation

Directly probing structure dynamics at metal/oxide interfaces has been a major challenge due to their buried nature.Using environmental transmission electron microscopy,here we report observations of the in-place formation of Cu 2 O/Cu interfaces via the oxidation of Cu, and subsequently probe the atomic mechanisms by which interfacial transformation and grain rotation occur at the interfaces during reduction in an H 2 gas environment. The Cu 2 O→Cu transformation is observed to occur initially along the Cu 2 O/Cu interface in a layer-by-layer manner.The accumulation of oxygen vacancies at the Cu 2 O/Cu interface drives the collapse of the Cu 2 O lattice near the interface region, which results in a tilted Cu 2 O/Cu interface with concomitant Cu 2 O island rotation. Lastly, these results provide unprecedented microscopic detail regarding the redox reactions of supported oxides,which differs fundamentally from the reduction of bulk or isolated oxides that requires the formation of new interfaces between the parent oxide and the reduced phase.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Effect of moisture on the traction-separation behavior of cellulose nanocrystal interfaces

Interfaces and stress transfer between cellulose nanocrystals (CNCs) dictate the mechanical properties of hierarchical cellulose materials such as neat films and nanocomposites. An interesting question that remains is how the behavior of these interfaces changes due to environmental stimuli, most notably moisture. We present analyses on the traction-separation behavior between Iβ CNC elementary fibrils, providing insight into how the presence of a single atomic layer of water at these interfaces can drastically change the mechanical behavior. We find that molecular water at the interface between hydrophilic CNC surfaces has a negligible effect on the tensile separation adhesion energy. However, when water cannot hydrogen bond easily to the surface (i.e., hydrophobic surface), it tends to maintain hydrogen bonds with other water molecules across the interface and form a capillary bridge that serves to increase the energy required to separate the crystals. Under shear loading, water lowers the energy barriers to sliding by reducing the atomic friction and consequently the interlayer shear modulus between crystals. Our simulations indicate that these nanoscale interfaces and physical phenomena such as interfacial adhesion, interlayer shear properties, and stick-slip friction behavior can be drastically altered by the presence of water.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

Mineral–Water Interface Structure of Xenotime (YPO 4 ) {100}

Crystal truncation rod (CTR) measurements and density functional theory (DFT) calculations were performed to determine the atomic structure of the mineral–water interface of the {100} surface of xenotime (nominally YPO 4 ). This mineral is important, because it incorporates a variety of rare earth elements (REEs) in its crystal structure. REEs are critical materials necessary for a variety of renewable and energy efficient technologies. Current beneficiation techniques are not highly selective for REE ore minerals, and large amounts go to waste; this is a first step toward designing more efficient beneficiation. Evidence is found for minor relaxation of the surface within the topmost monolayer with little or no relaxation in subsurface layers. Justification for ordered water at the interface is found, where water binds to surface cations and donates hydrogen bonds to surface phosphates. The average bond lengths between cations and oxygens on water are 228 pm in the best fit to the CTR data, versus 243 and 251 pm for the DFT. No agreement on water positions bound to surface phosphates is obtained. Altogether, the findings suggest that ligands used in beneficiation with a single anionic headgroup, such as fatty acids, will have limited selectivity for xenotime relative to undesirable minerals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Four High-Temperature Ferromagnets in the Hf–Fe–Sn System

We report the synthesis and characterization of four new ferromagnetic compounds discovered using Sn flux: Hf1.823(16)Fe5Sn3.815(14), HfFe2-xSnx, and two polymorphs of Hf1-xFe2Snx. All are closely related to HfFe2 Laves phase parent structures. HfFe2-xSnx (x approximate to 0.3-0.4) adopts the MgZn2-type (C14) crystal structure, whereas Hf1-xFe2Snx (x approximate to 0.1-0.4) adopts both the MgCu2-type (C15), and MgNi2-type (C36) structures. They crystallize in P6(3)/mmc, Fd3m, and P6(3)/mmc, respectively, with measured unit-cell parameters of a = 4.9238(7) angstrom and c = 7.9643(12) angstrom; a = 7.068(2) angstrom; and a = 4.9944(4) angstrom and c = 16.2604(15) angstrom, although phase width leads to a range of unit cell edge lengths. Hf1.823(16)Fe5Sn3.815(14) adopts a more complicated, incommensurately modulated structure in the superspace group Xmmm(00 gamma)000 with an orthorhombic subcell a = 9.7034(12) angstrom, b = 16.823(2) angstrom, and c = 8.4473(10) angstrom, three centering vectors of (1/2 0 0 1/2), (0 1/2 0 1/2), and (1/2 1/2 0 0), and a single-component modulation vector q = 0.2768(8)c*. The structure is composed of alternating slabs of the Fe-bonded Kagome nets observed in the HfFe2 parent structures alternated with Sn-rich Th2Zn17-type slabs, with Hf atoms primarily occurring at the interfaces between the slabs. All four compounds are ferromagnetic metals at room temperature, with Curie temperatures ranging from 467(2) to 658(2) K. Their coercive fields are remarkably low, between 2(1) and 15(2) Oe. Interestingly, in two of three cases the addition of nonmagnetic Sn atoms in place of magnetic Hf or Fe atoms in the HfFe2 structure seems to strengthen rather than weaken magnetic coupling and increase TC. Fits to electrical resistivity data for the compound suggest that electron scattering in the Laves phase polymorphs shows substantial contributions from electron-magnon and/or electron-electron scattering, while the electrical behavior of Hf1.823(16)Fe5Sn3.815(14) is dominated by electron-phonon scattering, as is the case in most metals.

Calta, Nicholas P.↗
DOE OSTI2015

Glide dislocation nucleation from dislocation nodes at semi-coherent {111} Cu–Ni interfaces

Using atomistic simulations and dislocation theory on a model system of semi-coherent {1 1 1} interfaces, we show that misfit dislocation nodes adopt multiple atomic arrangements corresponding to the creation and redistribution of excess volume at the nodes. We identified four distinctive node structures: volume-smeared nodes with (i) spiral or (ii) straight dislocation patterns, and volume-condensed nodes with (iii) triangular or (iv) hexagonal dislocation patterns. Volume-smeared nodes contain interfacial dislocations lying in the Cu–Ni interface but volume-condensed nodes contain two sets of interfacial dislocations in the two adjacent interfaces and jogs across the atomic layer between the two adjacent interfaces. Finally, under biaxial tension/compression applied parallel to the interface, we show that the nucleation of lattice dislocations is preferred at the nodes and is correlated with the reduction of excess volume at the nodes.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Delocalized electrons in atomic and molecular nanoclusters

The aim of the award (Program director: Dr. Mark Pederson) was to facilitate the attendance of researchers, students, and postdocs from the U.S. at the international workshop co-organized by the applicant. The award succeeded in making it possible for a number of US attendees to present their work and participate in the meeting, which was a significant event in the research community at the interdisciplinary interface of physical chemistry, nanoscience, atomic and molecular physics, condensed matter physics, and spectroscopy. The workshop did not issue proceedings, but the present report includes present the schedule, the abstracts, and the attendance list of the July 2016 Workshop. DOE sponsorship is gratefully acknowledged in the program.

74 ATOMIC AND MOLECULAR PHYSICS↗